Currently, activated coke is widely used in the removal of multiple pollutants from industrial flue gas. In this paper, a series of novel FexLayOz/AC catalysts was prepared by the incipient wetness impregnation for NH3-SCR denitrification reaction. The introduction of Fe-La bimetal oxides significantly improved the denitrification performance of activated coke at mid-high temperature, and 4% Fe0.3La0.7O1.5/AC exhibited a superior NOx conversion efficiency of 90.1% at 400 °C. The catalysts were further characterized by BET, SEM, XRD, Raman, EPR, XPS, FTIR, NH3-TPD, H2-TPR, et al., whose results showed that the perovskite-type oxide of LaFeO3 and oxygen vacancies were produced on the catalysts’ surfaces during roasting. Fe-La doping enhanced the amount of acid sites (mainly Lewis and other stronger acid sites) and the content of multifarious oxygen species, which were beneficial for NOx removal at mid-high temperature. Moreover, it was investigated that the effect of released CO from activated coke at mid-high temperature on the NOx removal through the lifetime test, in which it was found that a large amount of CO produced by pyrolysis of activated coke could promote the NOx removal, and long-term escaping of CO on the activated coke carrier did not have a significant negative impact on catalytic performance. The results of the TG-IR test showed that volatile matter is released from the activated coke while TG results showed that the weight loss rate of 4% Fe0.3La0.7O1.5/AC only was 0.0015~0.007%/min at 300–400 °C. Hence, 4% Fe0.3La0.7O1.5/AC had excellent thermal stability and denitrification performance to be continuously used at mid-high temperature. Finally, the mechanisms were proposed on the basis of experiments and characterization results.
• Fe(III) accepted the most electrons from organics, followed by NO3‒, SO42‒, and O2.• The electrons accepted by SO42‒ could be stored in the solid AVS, FeS2-S, and S0.• The autotrophic denitrification driven by solid S had two-phase characteristics.• A conceptual model involving electron acceptance, storage, and donation was built.• S cycle transferred electrons between organics and NO3‒ with an efficiency of 15%. A constructed wetland microcosm was employed to investigate the sulfur cycle-mediated electron transfer between carbon and nitrate. Sulfate accepted electrons from organics at the average rate of 0.84 mol/(m3·d) through sulfate reduction, which accounted for 20.0% of the electron input rate. The remainder of the electrons derived from organics were accepted by dissolved oxygen (2.6%), nitrate (26.8%), and iron(III) (39.9%). The sulfide produced from sulfate reduction was transformed into acid-volatile sulfide, pyrite, and elemental sulfur, which were deposited in the substratum, storing electrons in the microcosm at the average rate of 0.52 mol/(m3·d). In the presence of nitrate, the acid-volatile and elemental sulfur were oxidized to sulfate, donating electrons at the average rate of 0.14 mol/(m3·d) and driving autotrophic denitrification at the average rate of 0.30 g N/(m3·d). The overall electron transfer efficiency of the sulfur cycle for autotrophic denitrification was 15.3%. A mass balance assessment indicated that approximately 50% of the input sulfur was discharged from the microcosm, and the remainder was removed through deposition (49%) and plant uptake (1%). Dominant sulfate-reducing (i.e., Desulfovirga, Desulforhopalus, Desulfatitalea, and Desulfatirhabdium) and sulfur-oxidizing bacteria (i.e., Thiohalobacter, Thiobacillus, Sulfuritalea, and Sulfurisoma), which jointly fulfilled a sustainable sulfur cycle, were identified. These results improved understanding of electron transfers among carbon, nitrogen, and sulfur cycles in constructed wetlands, and are of engineering significance. 相似文献
This first nationwide survey was conducted to evaluate the overall performance of the circulating fluidized bed (CFB) incineration of municipal solid waste (MSW) in 2014-2015 in China. Total 23 CFB incineration power plants were evaluated. The data for monthly average flue gas emission of particles, CO, NOx, SO2 and HCl were collected over 12 consecutive months. The data were analyzed to assess the overall performance of CFB incineration by applying the Mahalanobis distance as a multivariate outlier detection method. Although the flue gas emission parameters had met the Chinese national emission standards, there were 11 total outliers (abnormal behavior) detected in 6 out of 23 CFB incineration power plants from the perspective of the MSWincineration performance. The results demonstrate that it is more important for a better performance of CFBs to reduce the frequencies of the MSW load changes, rather than the magnitudes of the MSW load changes, particularly reducing the frequencies in the range of 10% and more of the load changes, under the same and stable conditions. Furthermore, the overloading occurs more often than the underloading during the operation of the CFB incineration power plants in China. The frequent overloading is 0% to 30% of the designed capacity. To achieve the stable performance of CFBs in practice, an appropriately designed MSW storage capacity is suggested to build in a plant to buffer and reduce the frequency of the load changes. 相似文献
Water eutrophication in subtropical regions of southern China threatens watershed health and is of major concern. However, annual phosphorus (P) loading and its dominant causes are still unclear, especially at the watershed scale. In this study, we investigated dynamic P loadings and associated factors (e.g., land use, livestock production, and runoff depth) in ten watersheds that varied in area from 9 to 5,212 ha in a hilly area of Hunan Province, China. A flowmeter was installed at the outlet of each watershed, and total P (TP) and soluble P (SP) concentrations were monitored periodically from June 2010 to October 2012. The results showed that annual P loadings (APLs) in the ten watersheds ranged from 22.8 to 247.8 kg P/km2 and that P loss primarily occurred from April to June of each year during the main rainfall season in the study area. In addition, the average eutrophication (>0.05 mg P/L) ratio for stream waters was 86.7 % during the study period, which was indicative of a potentially serious condition for the local water environments. Annual P loadings were linearly related to livestock density (LD; R?=?0.92, p?<?0.01), whereas the eutrophication ratio of stream water was significantly (p?<?0.05) correlated with LD (R?=?0.61), percentage cropland (R?=?0.71), and percentage forest cover (R?=??0.68). Thus, it is concluded that the control of livestock production has the greatest potential for reducing P loadings in watersheds in this subtropical area. This will be beneficial to the amelioration and protection of local environment. 相似文献